Lithiated Prussian blue analogues as positive electrode active materials for stable non-aqueous lithium-ion batteries

Abstract
Prussian blue analogues (PBAs) are appealing active materials for post-lithium electrochemical energy storage. However, PBAs are not generally suitable for non-aqueous Li-ion storage due to their instability upon prolonged cycling. Herein, we assess the feasibility of PBAs with various lithium content for non-aqueous Li-ion storage. We determine the crystal structure of the lithiated PBAs via neutron powder diffraction measurements and investigate the influence of water on structural stability and Li-ion migration through operando X-ray diffraction measurements and bond valence simulations. Furthermore, we demonstrate that a positive electrode containing Li2-xFeFe(CN)6⋅nH2O (0 ≤ x ≤ 2) active material coupled with a Li metal electrode and a LiPF6-containing organic-based electrolyte in coin cell configuration delivers an initial discharge capacity of 142 mAh g−1 at 19 mA g−1 and a discharge capacity retention of 80.7% after 1000 cycles at 1.9 A g−1. By replacing the lithium metal with a graphite-based negative electrode, we also report a coin cell capable of cycling for more than 370 cycles at 190 mA g−1 with a stable discharge capacity of about 105 mAh g−1 and a discharge capacity retention of 98% at 25 °C. © The Authors CC 4.0
Description
Keywords
Lithium, Electrodes, Lithium ion batteries, X-ray diffraction, Measuring instruments, Materials, Iron
Citation
Zhang, Z., Avdeev, M., Chen, H., Yin, W., Kan, W. H., & He, G. (2022). Lithiated Prussian blue analogues as positive electrode active materials for stable non-aqueous lithium-ion batteries. Nature Communications, 13(1), 7790. doi:10.1038/s41467-022-35376-1
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